Traditional neural interfaces are limited in functionality and longevity due to their lack of biocompatibility. A new class of dynamic materials known as shape memory polymers has been introduced as an alternative to conventional substrates for neural interfaces. Using photolithography, gold electrodes are deposited on a smart, softening thiol-ene/acrylate polymer substrate to achieve a reliable communication platform for recording neural activity. Recording electrodes have been designed with geometric surface areas ranging from 177 to 2.5 million square microns. The different-sized sites allow for unique, tailorable electrochemical properties for each probe. The substrate softens at body temperature with minimal fluid uptake and without dramatic change in electrochemical properties. Under prolonged exposure to simulated physiological conditions, the 177 square micron device has been proven capable of maintaining its electrical integrity, with a typical impedance shift (at 1 kHz) from 1.65±0.95 to 0.33±0.19 MΩ after 30 days.